Neutron Coincidence Measurements of Uranium-233 Oxide
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Distinguishing fissile uranium isotopes using an active well neutron coincidence counter
Proposed thorium-based nuclear fuel cycles are likely to require quantification and verification of 233 U within nuclear material. Because of their similar fission cross sections, active neutron nondestructive assay (NDA) systems may respond similarly to 233 U and 235 U. Traditional safeguards equipment has been optimized for 235 U and 238 U quantification associated with conventional uranium/plutonium fuel cycles and may not be directly applicable to 233 U quantification when mixed with other actinides. This work used models of the large volume active well coincidence counter (LV-AWCC) at Oak Ridge National Laboratory to evaluate the performance of this neutron NDA system to differentiate fissile uranium isotopes. The models were developed to simulate NDA system performance in response to a number of triangular radiation signature training device sources within the central cavity or well. This work predicted that the LV-AWCC can effectively differentiate 233 U from 235 U in certain modes of operation. In active mode, the LV-AWCC with the cadmium liner results in different doubles count rates between the fissile isotopes for a given fissile uranium mass. Without the cadmium liner, the uranium isotopes provide a statistically indistinguishable doubles count rate response for the fissile masses considered in this work (up to approximately 150 g). The cadmium liner serves to harden the neutron interrogation spectrum, which better exploits the notable difference in the 233 U and 235 U fission cross sections at approximately 1 eV. In passive mode, the two fissile isotopes exhibit different doubles and singles count rates regardless of liner presence because the passive source strength of 233 U is approximately 2 orders of magnitude stronger than that of 235 U due to the shorter half-life and correspondingly higher (α, n) yield. We conclude that using neutron interrogation in the LV-AWCC, two measurements are needed to quantify 233 U content in mixed uranium items. The first measurement is used to determine the total fissile uranium mass using a mode that cannot distinguish fissile isotopes (i.e., where a similar response is observed for both fissile uranium isotopes such as active doubles without cadmium or using a thermal neutron interrogation source). In conclusion, the second measurement is used to determine the 233 U content by using a differentiating technique (e.g., passive doubles, passive doubles to singles ratio, active doubles with cadmium).
46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
Comparison of active interrogation methods for source location in a scattering and absorbing medium, consisting of PGNAA, and an AmBe quasi-forward biased directional source
Source location of Special Nuclear Material (SNM) encompassing 95% 235 U and 239 Pu is identified by utilizing a directional source from Patent No: US20190013109A1 using Prompt Gamma Neutron Activation Analysis (PGNAA) and neutron spectroscopy simulated with Monte-Carlo N-Particle transport 6.2 (MCNP). BC-408, HPGe, LaBr 3 detector arrays were used to identify the location of the SNM using total counts incident on each detector, and PGNAA photopeaks from HPGe and LaBr 3 detector arrays in a polyethylene shield. The conducted simulations varied the volume and location of the SNM in the MCNP input files to observe how the source location method behaved. PGNAA photopeaks used for source identification include 61 keV from fission, 2.223 MeV prompt gamma from hydrogen, 511 keV annihilation, and a single and double escape peaks from the prompt gamma interaction from hydrogen. The capabilities of each detector systems to acquire well resolved photopeaks with a 1% relative error or less, and total relative error for F4 and F8 tallies were less than 0.015% relative error. Source predictions of the SNM with uneven amounts of polyethylene shielding between the source and detectors was observed to overpredict and give invalid source location predictions. Source locations of the SNM with even amounts of polyethylene material between the source and each detector were found to be valid. With a 1 Ci 241 Am source activity, it was determined that 1630 s were needed to obtain the results for each detector system with the quasi-forward directional AmBe source. Coupling source and material identification together would increase acquisition time but would only require one system to determine.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Pulsed-Neutron Experiments at the Inherently Safe Subcritical Assembly
The pulsed neutron technique is a powerful, dynamic method to assay the reactivity of a multiplying system. This work presents the novel application of the pulsed neutron technique to the Inherently Safe Subcritical Assembly, an experimental configuration accepted by the International Criticality Safety Benchmark Evaluation Project Handbook. The experiments were replicated with COG11.3, a continuous-energy Monte Carlo code. The pulsed neutron data were analyzed using the Sjöstrand and Gozani area-ratio methods and by extracting the prompt neutron decay constant. Subsequent static k-eigenvalue and 𝛼-eigenvalue simulations were also performed for the same configurations. Neutron detector dead-time effects from the experiments were corrected using the Backwards Extrapolation Method and shown to have a negligible impact on the estimated reactivities. The results highlight that capturing time-dependent effects like delayed neutron precursor buildup are essential to accurately reproduce experimental results. They also highlight the importance of shielding the detectors from generator source neutrons in deeply subcritical configurations.
21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗
Improved field assessments of chemicals and explosives using high-resolution gamma-ray spectroscopy with a tagged neutron interrogation system
A field-portable tagged neutron interrogation system is being developed for detection of explosives and chemical warfare agents by prompt γ-ray neutron activation analysis. The system combines an associated particle imaging deuterium-tritium neutron generator with a high-purity germanium γ-ray detector. Fine spatial resolution neutron and α detectors enable precise mapping of characteristic γ-ray emission distributions onto high-clarity neutron radiographic images. A narrow coincidence gate associated with each tagged neutron ensures a large signal-to-background ratio, thus significantly improving sensitivity to the chemical compositions of the items being assessed. Recent experimental results recorded from test objects involving mock explosives and other chemicals are presented.
Bucher, Brian [Idaho National Laboratory (INL)]↗
Improved field assessments of chemicals and explosives using high-resolution gamma-ray spectroscopy with a tagged neutron interrogation system
A fi eld-portable tagged neutron interrogation system is being developed for detection of explosives and chemical warfare agents by prompt gamma-ray neutron activation analysis. The system combines an associated particle imaging deuterium-tritium neutron generator with a high-purity germanium gamma-ray detector. Fine spatial resolution neutron and alpha detectors enable precise mapping of characteristic gamma-ray emission distributions onto high-clarity neutron radiographic images. A narrow coincidence gate associated with each tagged neutron ensures a large signal-to-background ratio, thus signifi cantly improving sensitivity to the chemical compositions of the items being assessed. Recent experimental results recorded from test objects involving mock explosives and other chemicals are presented.
46 - INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AN↗
Improved field assessments of chemicals and explosives using high-resolution gamma-ray spectroscopy with a tagged neutron interrogation system
A fi eld-portable tagged neutron interrogation system is being developed for detection of explosives and chemical warfare agents by prompt gamma-ray neutron activation analysis. The system combines an associated particle imaging deuterium-tritium neutron generator with a high-purity germanium gamma-ray detector. Fine spatial resolution neutron and alpha detectors enable precise mapping of characteristic gamma-ray emission distributions onto high-clarity neutron radiographic images. A narrow coincidence gate associated with each tagged neutron ensures a large signal-to-background ratio, thus signifi cantly improving sensitivity to the chemical compositions of the items being assessed. Recent experimental results recorded from test objects involving mock explosives and other chemicals are presented.
46 - INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AN↗
New NDA Methods for Thorium Fuel Cycle Safeguards (Final Report)
This project developed portable Neutron Resonance Transmission Analysis (pNRTA) as a new non-destructive assay (NDA) method for thorium fuel cycles safeguards and other applications where multiple isotopes must be measured when present together. pNRTA leverages epithermal neutron resonances to assay multiple safeguards-relevant isotopes (e.g., 233 U and 235 U) when they are present together in a sample. Existing techniques are challenged by this task, driving the need for new active interrogation methods. With selected detectors, pNRTA works in high gamma-ray backgrounds from fission and activation products and 232 U progeny expected in thorium fuel cycle samples. This project leveraged a pNRTA system developed at Pacific Northwest National Laboratory (PNNL) and collaboration with the Massachusetts Institute of Technology (MIT). The system uses a commercially available deuterium-tritium (DT) neutron generator at short standoff (2 m). Key achievements in this project included: first-of-a-kind pNRTA quantitative measurements of 233 U oxide samples, an assessment of neutron detector technologies suitable for pNRTA in high gamma-ray background environments, experimentally demonstrating quantitative assay of samples containing 233 U and 235 U, and modeling studies showing the applicability of pNRTA to a wide range of material forms. Further, a custom algorithm was developed at MIT, which provided mean bias of 9% and relative standard deviation of 36% in assaying 233 U, 235 U, 238 U, and 232 Th content in eight measured samples. These outcomes form a solid technical basis for pNRTA as a new promising capability for international safeguards verification that is portable, non-destructive, quantitative, and isotopic specific.
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
New NDA Methods for Thorium Fuel Cycle Safeguards (Mid-Project Report)
This project is developing new Non-Destructive Assay (NDA) safeguards techniques for emergent thorium fuel cycles based on Neutron Resonance Transmission Analysis (NRTA), which can assay 233 U and 235 U when they are present together in a sample with potentially high gamma-ray backgrounds from fission products and 232 U. Existing passive techniques face large challenges for this task so new active interrogation methods are needed. This effort is also exploring how gamma-ray signatures can complement NRTA for enhanced assayed performance. This project leverages an NRTA system being developed at PNNL in collaboration with MIT, which uses a commercially available deuterium-tritium neutron generator at short standoff (~2 m). We aim to assess the feasibility and performance of these new NDA techniques for the range of relevant samples in thorium fuel cycles. Key advancements described in this mid-project report include NRTA system design for thorium safeguards measurements, characterization of 233 U oxide powder at PNNL, a survey of detector technologies suitable for NRTA in high gamma background environments, successful preliminary demonstration of a quantitative isotopic estimation algorithm, and first NRTA measurements of a thorium sample.
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
Multi-Modal, Multi-Energy Approach for Neutron Interrogation of Spent Fuel
Air Force War College Presentation at Nellis Air Force Base on March 25, 2021
73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
Sensitivity of the active neutron coincidence collar response during simulated and experimental fresh fuel assay
Verification of the fissile (and fertile) content in fresh nuclear fuel assemblies is conducted by the IAEA to enforce the Nuclear Non-Proliferation Treaty using the UNCL (Uranium Neutron Collar — Light Water Reactor Fuel). The UNCL uses an uncorrelated AmLi neutron source to interrogate the fuel, producing a signal of coincident fission neutrons (Doubles rate) used to assay 235 U content of the fuel. The cost of producing calibration assemblies and limited availability of diverse commercial assemblies at any one time historically restricted the ability to explore the full parameter space experimentally. Monte Carlo simulations can overcome this, but introduce additional sources of uncertainty. In this work, the sensitivity of simulations and measurements to various parameters is assessed for a reference 1616 PWR assembly of uniform 3.2% enrichment. Uncertainty contributions in this evaluation include: simulated AmLi neutron source spectrum, AmLi neutron emission rate, AmLi anisotropicity, high density polyethylene (HDPE) density, the precise position of the fuel assembly within the detector, and experimentally the statistical uncertainty. The overall total systematic uncertainty estimate for the simulation of the absolute/relative Doubles rates responses are estimated to be approximately 2.0%/1.5%, and for experimental measurements systematic uncertainty reduces to 1.1%. This analysis supports further work using the relative Doubles rates in place of measurements for updating and extending the UNCL analysis methodology as systematic uncertainty is reasonably small.
46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
Observation of an Intermediate to H 2 Binding in a Metal–Organic Framework
Coordinatively unsaturated metal sites within certain zeolites and metal–organic frameworks can strongly adsorb a wide array of substrates. While many classical examples involve electron-poor metal cations that interact with adsorbates largely through physical interactions, unsaturated electron-rich metal centers housed within porous frameworks can often chemisorb guests amenable to redox activity or covalent bond formation. Despite the promise that materials bearing such sites hold in addressing myriad challenges in gas separations and storage, very few studies have directly interrogated mechanisms of chemisorption at open metal sites within porous frameworks. Here, we show that nondissociative chemisorption of H 2 at the trigonal pyramidal Cu + sites in the metal–organic framework Cu I -MFU- 4 l occurs via the intermediacy of a metastable physisorbed precursor species. In situ powder neutron diffraction experiments enable crystallographic characterization of this intermediate, the first time that this has been accomplished for any material. Evidence for a precursor intermediate is also afforded from temperature-programmed desorption and density functional theory calculations. Here, the activation barrier separating the precursor species from the chemisorbed state is shown to correlate with a change in the Cu + coordination environment that enhances p-backbonding with H 2 . Ultimately, these findings demonstrate that adsorption at framework metal sites does not always follow a concerted pathway and underscore the importance of probing kinetics in the design of next-generation adsorbents.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Planetary Geochemistry Techniques: Probing In-Situ with Neutron and Gamma Rays (PING) Instrument
The Probing In situ with Neutrons and Gamma rays (PING) instrument is a promising planetary science application of the active neutron-gamma ray technology so successfully used in oil field well logging and mineral exploration on Earth. The objective of our technology development program at NASA Goddard Space Flight Center's (NASA/GSFC) Astrochemistry Laboratory is to extend the application of neutron interrogation techniques to landed in situ planetary composition measurements by using a 14 MeV Pulsed Neutron Generator (PNG) combined with neutron and gamma ray detectors, to probe the surface and subsurface of planetary bodies without the need to drill. We are thus working to bring the PING instrument to the point where it can be flown on a variety of surface lander or rover missions to the Moon, Mars, Venus, asteroids, comets and the satellites of the outer planets.
Parsons, A.↗
Active Interrogation of the Snyder Shells using a SEA-7 Betatron
The shielded highly enriched uranium (HEU) problem is one that still needs to be addressed. As a first step towards a solution, the Snyder shells (depleted uranium) were actively interrogated with a SEA-7 betatron in various configurations using an MC15 as a detector. These configurations include masses from 0.55 to 5.1 kg, as well as 5.1 kg in a steel container. A strong electromagnetic field (EMF) background was identified in previous work, but the results in this work show all configurations produce a signal well above the background. An initial simulation capability was developed that produces the expected flux profile from the SEA-7 betatron, but further work needs to be done to determine the magnitude of the flux via a combination of experiment and simulation validation. Depleted uranium generally produces more neutrons than HEU, so additional future work will need to include similar measurements of HEU to confirm similar performance of the technique. Additionally the EMF background needs to be better characterized as a function of distance and angle from the SEA-7 source and mitigation techniques explored.
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
An Artificial Neural Network System for Photon-Based Active Interrogation Applications
Active interrogation (AI) is a promising technique to detect shielded special nuclear materials (SNMs). At the University of Michigan, we are developing a photon-based AI system that uses bremsstrahlung radiation from an electron linear accelerator (linac) as an ionizing source and stilbene organic scintillating detectors for neutron detection. Stilbene scintillators are sensitive to fast neutrons and photons and have excellent pulse shape discrimination (PSD) capabilities. The traditional charge integration (CI) method commonly used for PSD analysis eliminates piled-up pulses and relies on a particle discrimination line to separate neutrons and photons. The presence of the intense photon flux during AI creates a significant number of piled-up events in the stilbene scintillator, thereby posing a great challenge to the traditional CI method. Identifying true single neutron pulses becomes challenging due to the presence of a pile-up cloud and overlapping neutron, photon and pile-up clouds in the PSD analysis. To mitigate the effect of pulse pile up and identify true single neutron pulses from stilbene scintillators, an artificial neural network (ANN) system is developed. The developed ANN system identifies single neutron pulses and neutron-photon combinations from piled-up events. The results obtained from a 252Cf measurement in the presence of the intense photon flux show that the developed ANN system outperforms the traditional CI method. Since many piled-up events lie above the particle discrimination line, they get misclassified as neutrons by the traditional CI method resulting in 25% overestimation of the net neutron count rate during the linac pulse. The overall net neutron count rate (single and restored neutrons) during the linac pulse, estimated by the ANN system is 60% of the ground truth. Energy spectroscopy of the ANN attributed single neutron pulses further provides evidence on the detection of prompt fission neutrons from the 252Cf fission source.
42 ENGINEERING↗
Active Irradiation Testing of Temperature Sensing Capability of Clad Sapphire Optical Fibers with Type 2 Bragg Gratings using Optical Backscatter Reflectometry
This work investigated the temperature-sensing capabilities of Type II fiber Bragg gratings (FBGs) inscribed in sapphire optical fiber in the Ohio State University Research Reactor (OSURR). A Luna Innovations 4600 optical backscatter reflectometer (OBR) was used to interrogate FBGs in three sapphire optical fibers with an internal cladding that was developed by Ohio State. The sapphire fibers were fusion-spliced to silica lead fibers. In addition to the sapphire fibers, two silica fibers with the same Type II FBGs were included in the experiment as a reference. The fiber-based sensors were irradiated in the Central Irradiation Facility (CIF) of the OSURR for a total of 40 hours over 5 days at a reactor power of 450 kW, resulting in a total neutron fluence of approximately 2.5 × 10 18 n/cm 2 and a gamma dose of approximately 3.48 Grad. Two K-type thermocouples were included within the rig: one at the core centerline and the other 12 inches above the top of the core. The temperature was not actively controlled, but the thermocouples were used to provide a reference to which the fiber-based temperature measurements could be compared.
36 MATERIALS SCIENCE↗
12 C(p,p') 12 C Reaction ( E p =19.5–30 MeV) for Active Interrogation of Special Nuclear Material
Passive detection of special nuclear material (SNM) is challenging due to its inherently low rate of spontaneous emission of penetrating radiation, the relative ease of shielding, and the fluctuating and frequently overwhelming background. Active interrogation, the use of external radiation to increase the emission rate of characteristic radiation from SNM, has long been considered to be a promising method to overcome those challenges. Current active-interrogation systems that incorporate radiography tend to use bremsstrahlung beams, which can deliver high radiation doses. Low-energy ion-driven nuclear reactions that produce multiple monoenergetic photons may be used as an alternative. The 12 C ( p , p ' ) 12 C reaction is one such reaction that could produce large yields of highly penetrating 4.4- and 15.1-MeV gamma rays. This reaction does not directly produce neutrons below the approximately 19.7 MeV threshold, and the 15.1-MeV gamma-ray line is well matched to the photofission cross section of 235 U and 238 U . In this article, we report the measurements of thick-target gamma-ray yields at 4.4 and 15.1 MeV from the 12 C ( p , p ' ) 12 C reaction at proton energies of 19.5, 25, and 30 MeV. Measurements are made with two 3 -in. EJ-309 cylindrical liquid scintillation detectors and thermoluminescent dosimeters placed at 0 ° and 90 ° , with an additional 1.5 -in. Na I ( Tl ) cylindrical scintillation detector at 0 ° . We estimate the highest yields of the 4.4- and 15.1-MeV gamma rays of 1.65 × 10 10 and 4.47 × 10 8 sr - 1 μ C - 1 at a proton energy of 30 MeV, respectively. The yields in all experimental configurations are greater than in a comparable deuteron-driven reaction that produces the same gamma-ray energies— 11 B ( d , n γ ) 12 C . However, a significant increase of the neutron radiation dose accompanies the proton energy increase from 19.5 to 30 MeV.
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
Environmental Contributions to Proton Sharing in Protein Low-Barrier Hydrogen Bonds
Hydrogen bonds (H-bonds) are central to biomolecular structure and dynamics. Although H-bonds are typically characterized by well-defined proton positions, proton delocalization has been proposed to play a role in facilitating enzyme catalysis and allostery in some systems. Experimentally locating protons is difficult, hampering the study of proton mobility in H-bonds. We used neutron crystallography, atomic resolution X-ray bond length analysis, and large quantum mechanics/molecular mechanics-Born–Oppenheimer molecular dynamics (QM/MM-BOMD) simulations to comprehensively characterize the shared proton/deuteron in a Glu–Asp low-barrier hydrogen bond (LBHB) in the bacterial protein YajL that is a conventional H-bond in the homologous disease-associated human protein DJ-1. X-ray bond length analysis of protiated and perdeuterated DJ-1 and YajL shows no significant effect of deuteron substitution on these carboxylic acid-carboxylate H-bonds but does reveal an effect at the active site glutamic acid near a cysteine thiolate. Residues in an H-bonded network that might favor LBHB formation in YajL were interrogated by the mutation of homologous residues in DJ-1. A distal DJ-1 substitution increases proton delocalization in the Glu–Asp H-bond, demonstrating that mutations within extended H-bond networks can modulate proton transfer barriers in carboxylic acid-carboxylate H-bonds. In addition, proton mobility in the H-bond is correlated with dimer-spanning motions in the QM/MM-BOMD simulations of YajL and DJ-1. Our results show that proton delocalization can be tuned using combined bioinformatic, structural, and computational information, opening the possibility of using engineered proton delocalization as a probe of H-bonding environments and as a tool to test hypotheses about LBHB function.
Lin, Jiusheng [University of Nebraska, Lincoln, NE↗